Abstract
We demonstrate a scalable and energy-efficient hollow fiber membrane contactor (HFMC)-based process using a green solvent for CO2 capture. This process uses a deep eutectic solvent (DES) in an HFMC to provide close interfacial interactions and contact between the DES and CO2. This approach overcomes disadvantages associated with direct absorption in DES and could potentially be applied to a variety of solvent-based CO2 capture methods. Commercial low-cost polymer hollow fiber membranes (e.g., microporous polypropylene) were evaluated for CO2 capture with reline, a prototypical DES. Single-gas measurements showed that the DES-based polypropylene HFMC can capture and separate CO2 while rejecting N2. From a mixed gas containing 50 mol % N2 and 50 mol % CO2, the DES-based HFMC separated CO2 with a purity of 96.9 mol %. The effect of several process parameters including solvent flow rate, pressure, and temperature on the CO2 separation performance was studied. The flux of the recovered CO2 was 67.43 mmole/m2/h at a feed pressure of 4 bar. In situ Fourier transform infrared (FTIR) measurements combined with density functional theory (DFT)-based molecular dynamics simulations revealed that reline absorbs CO2 by physical absorption without forming a new chemical compound, and CO2 separation by reline occurs via the pressure swing mechanism. This research provides fundamental insights about physical solvent-based separation processes and a pathway toward practical deployment.
Original language | English |
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Pages (from-to) | 4455-4465 |
Number of pages | 11 |
Journal | Industrial and Engineering Chemistry Research |
Volume | 62 |
Issue number | 10 |
DOIs | |
State | Published - Mar 15 2023 |
Funding
The authors acknowledge the extensive support in experimental activities provided by Dale Adcock and Lawrence E. Powell. The authors thank Dale K. Hensley for SEM images. The authors also thank Anisur Rahman, Rajeev Kumar, Alexei Sokolov, Michelle Kidder, Priyesh Wagh, Nirupam Aich, and Amit Sengupta for their fruitful discussion. SEM imaging was conducted at ORNL’s Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility. Theoretical calculations used computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE) through allocation TG-DMR110037. This project is supported by the Laboratory Directed Research and Development Funding, Transformational Decarbonization Initiative, Oak Ridge National Laboratory. This manuscript has been authored by UT-Battelle LLC under contract no. DE-AC05-00OR22725 with the US Department of Energy. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). The authors acknowledge the extensive support in experimental activities provided by Dale Adcock and Lawrence E. Powell. The authors thank Dale K. Hensley for SEM images. The authors also thank Anisur Rahman, Rajeev Kumar, Alexei Sokolov, Michelle Kidder, Priyesh Wagh, Nirupam Aich, and Amit Sengupta for their fruitful discussion. SEM imaging was conducted at ORNL’s Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility. Theoretical calculations used computational resources of the Extreme Science and Engineering Discovery Environment (XSEDE) through allocation TG-DMR110037. This project is supported by the Laboratory Directed Research and Development Funding, Transformational Decarbonization Initiative, Oak Ridge National Laboratory. This manuscript has been authored by UT-Battelle LLC under contract no. DE-AC05-00OR22725 with the US Department of Energy. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).
Funders | Funder number |
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DOE Public Access Plan | |
Laboratory Directed Research | |
U.S. Department of Energy | |
Office of Science | |
Oak Ridge National Laboratory | |
UT-Battelle | DE-AC05-00OR22725 |